In the present paper, used cigarette filter ash was prepared and used as an active adsorbent to remove As(III) ions from aqueous solutions. The prepared adsorbent structure was identified by scanning electron microscopy analysis, Brunauer–Emmett–Teller method and energy-dispersive X-ray spectroscopy analysis. The influence of contact time, pH, adsorbent dose and initial concentration of As(III) on the removal of As(III) was assessed. Several isotherm models were checked to illustrate the adsorption equilibrium. The adsorption equilibrium data adapted well with the Langmuir isotherm model. The maximum adsorption capacity of 33.33 mg/g was acquired from the Langmuir isotherm. The calculated thermodynamic variables verified that the adsorption process is spontaneous and endothermic.